Ultrafast spectroscopy of shift-current in ferroelectric semiconductor Sn2P2S6

M. Sotome; M. Nakamura; J. Fujioka; M. Ogino; Y. Kaneko; T. Morimoto; Y. Zhang; M. Kawasaki; N. Nagaosa; Y. Tokura; N. Ogawa

doi:10.1063/1.5087960

Ultrafast spectroscopy of shift-current in ferroelectric semiconductor Sn₂P₂S₆

M. Sotome
, M. Nakamura
, J. Fujioka
, M. Ogino
, Y. Kaneko
, T. Morimoto
, Y. Zhang
, M. Kawasaki
, N. Nagaosa
, Y. Tokura
, N. Ogawa

Materials Theory

Research output: Contribution to journal › Article › peer-review

21 Scopus citations

Abstract

We report sub-picosecond photocarrier dynamics observed via emitted terahertz waves in a ferroelectric semiconductor Sn₂P₂S₆. Excitation photon energy, intensity and polarization dependences of the photocarrier dynamics testify that the ultrafast photocurrent originates from the shift-current under interband excitation. The photocurrent excitation spectrum shows a quantitative agreement with that derived from first-principles calculations with the Berry connection integrated, showing the shift-current to be a sensitive feature in ferroelectrics. The terahertz emission spectroscopy is a powerful tool to identify the intricate carrier dynamics under pulsed photoexcitation.

Original language	English
Article number	151101
Journal	Applied Physics Letters
Volume	114
Issue number	15
DOIs	https://doi.org/10.1063/1.5087960
State	Published - Apr 15 2019

Funding

We thank D. Maryenko, Y. Taguchi and M. Ueda for stimulating discussions. This research was supported by JSPS KAKENHI Grant Nos. 18K14155, 24224009, 16H00981, 16K13705, and 17H02914. M.N., J.F., and N.O. were supported by PRESTO, JST (JPMJPR16R5, JPMJPR15R5, and JPMJPR17I3, respectively). T.M. was supported by the Quantum Materials Program at LBNL funded by the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Y.Z. was supported by German Research Foundation (DFG) SFB 1143. The authors declare no conflict of interest. N.N. was supported by JST CREST Grant No. JPMJCR16F1, Japan, and JSPS KAKENHI Grant Nos. 18H03676 and 26103001.

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title = "Ultrafast spectroscopy of shift-current in ferroelectric semiconductor Sn2P2S6",

abstract = "We report sub-picosecond photocarrier dynamics observed via emitted terahertz waves in a ferroelectric semiconductor Sn2P2S6. Excitation photon energy, intensity and polarization dependences of the photocarrier dynamics testify that the ultrafast photocurrent originates from the shift-current under interband excitation. The photocurrent excitation spectrum shows a quantitative agreement with that derived from first-principles calculations with the Berry connection integrated, showing the shift-current to be a sensitive feature in ferroelectrics. The terahertz emission spectroscopy is a powerful tool to identify the intricate carrier dynamics under pulsed photoexcitation.",

author = "M. Sotome and M. Nakamura and J. Fujioka and M. Ogino and Y. Kaneko and T. Morimoto and Y. Zhang and M. Kawasaki and N. Nagaosa and Y. Tokura and N. Ogawa",

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AU - Sotome, M.

AU - Nakamura, M.

AU - Fujioka, J.

AU - Ogino, M.

AU - Kaneko, Y.

AU - Morimoto, T.

AU - Zhang, Y.

AU - Kawasaki, M.

AU - Nagaosa, N.

AU - Tokura, Y.

AU - Ogawa, N.

PY - 2019/4/15

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N2 - We report sub-picosecond photocarrier dynamics observed via emitted terahertz waves in a ferroelectric semiconductor Sn2P2S6. Excitation photon energy, intensity and polarization dependences of the photocarrier dynamics testify that the ultrafast photocurrent originates from the shift-current under interband excitation. The photocurrent excitation spectrum shows a quantitative agreement with that derived from first-principles calculations with the Berry connection integrated, showing the shift-current to be a sensitive feature in ferroelectrics. The terahertz emission spectroscopy is a powerful tool to identify the intricate carrier dynamics under pulsed photoexcitation.

AB - We report sub-picosecond photocarrier dynamics observed via emitted terahertz waves in a ferroelectric semiconductor Sn2P2S6. Excitation photon energy, intensity and polarization dependences of the photocarrier dynamics testify that the ultrafast photocurrent originates from the shift-current under interband excitation. The photocurrent excitation spectrum shows a quantitative agreement with that derived from first-principles calculations with the Berry connection integrated, showing the shift-current to be a sensitive feature in ferroelectrics. The terahertz emission spectroscopy is a powerful tool to identify the intricate carrier dynamics under pulsed photoexcitation.

UR - https://www.scopus.com/pages/publications/85064459163

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DO - 10.1063/1.5087960

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VL - 114

JO - Applied Physics Letters

JF - Applied Physics Letters

IS - 15

M1 - 151101

ER -

Ultrafast spectroscopy of shift-current in ferroelectric semiconductor Sn₂P₂S₆

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